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Accelerated discovery of CO2 electrocatalysts using active machine learning 期刊论文
NATURE, 2020, 581 (7807) : 178-+
作者:  Lan, Jun;  Ge, Jiwan;  Yu, Jinfang;  Shan, Sisi;  Zhou, Huan;  Fan, Shilong;  Zhang, Qi;  Shi, Xuanling;  Wang, Qisheng;  Zhang, Linqi;  Wang, Xinquan
收藏  |  浏览/下载:88/0  |  提交时间:2020/07/03

The rapid increase in global energy demand and the need to replace carbon dioxide (CO2)-emitting fossil fuels with renewable sources have driven interest in chemical storage of intermittent solar and wind energy(1,2). Particularly attractive is the electrochemical reduction of CO2 to chemical feedstocks, which uses both CO2 and renewable energy(3-8). Copper has been the predominant electrocatalyst for this reaction when aiming for more valuable multi-carbon products(9-16), and process improvements have been particularly notable when targeting ethylene. However, the energy efficiency and productivity (current density) achieved so far still fall below the values required to produce ethylene at cost-competitive prices. Here we describe Cu-Al electrocatalysts, identified using density functional theory calculations in combination with active machine learning, that efficiently reduce CO2 to ethylene with the highest Faradaic efficiency reported so far. This Faradaic efficiency of over 80 per cent (compared to about 66 per cent for pure Cu) is achieved at a current density of 400 milliamperes per square centimetre (at 1.5 volts versus a reversible hydrogen electrode) and a cathodic-side (half-cell) ethylene power conversion efficiency of 55 +/- 2 per cent at 150 milliamperes per square centimetre. We perform computational studies that suggest that the Cu-Al alloys provide multiple sites and surface orientations with near-optimal CO binding for both efficient and selective CO2 reduction(17). Furthermore, in situ X-ray absorption measurements reveal that Cu and Al enable a favourable Cu coordination environment that enhances C-C dimerization. These findings illustrate the value of computation and machine learning in guiding the experimental exploration of multi-metallic systems that go beyond the limitations of conventional single-metal electrocatalysts.


  
Accurate compound-specific C-14 dating of archaeological pottery vessels 期刊论文
NATURE, 2020, 580 (7804) : 506-+
作者:  Yin, Yafei;  Lu, J. Yuyang;  Zhang, Xuechun;  Shao, Wen;  Xu, Yanhui;  Li, Pan;  Hong, Yantao;  Cui, Li;  Shan, Ge;  Tian, Bin;  Zhang, Qiangfeng Cliff;  Shen, Xiaohua
收藏  |  浏览/下载:20/0  |  提交时间:2020/05/13

Pottery is one of the most commonly recovered artefacts from archaeological sites. Despite more than a century of relative dating based on typology and seriation(1), accurate dating of pottery using the radiocarbon dating method has proven extremely challenging owing to the limited survival of organic temper and unreliability of visible residues(2-4). Here we report a method to directly date archaeological pottery based on accelerator mass spectrometry analysis of C-14 in absorbed food residues using palmitic (C-16:0) and stearic (C-18:0) fatty acids purified by preparative gas chromatography(5-8). We present accurate compound-specific radiocarbon determinations of lipids extracted from pottery vessels, which were rigorously evaluated by comparison with dendrochronological dates(9,10) and inclusion in site and regional chronologies that contained previously determined radiocarbon dates on other materials(11-15). Notably, the compound-specific dates from each of the C-16:0 and C-18:0 fatty acids in pottery vessels provide an internal quality control of the results(6) and are entirely compatible with dates for other commonly dated materials. Accurate radiocarbon dating of pottery vessels can reveal: (1) the period of use of pottery  (2) the antiquity of organic residues, including when specific foodstuffs were exploited  (3) the chronology of sites in the absence of traditionally datable materials  and (4) direct verification of pottery typochronologies. Here we used the method to date the exploitation of dairy and carcass products in Neolithic vessels from Britain, Anatolia, central and western Europe, and Saharan Africa.


Using lipid residues absorbed in potsherds, the ages of pottery from various archaeological sites are determined and validated using sites for which the dates are well known from other methods.


  
Spin squeezing of 10(11) atoms by prediction and retrodiction measurements 期刊论文
NATURE, 2020, 581 (7807) : 159-+
作者:  Lan, Jun;  Ge, Jiwan;  Yu, Jinfang;  Shan, Sisi;  Zhou, Huan;  Fan, Shilong;  Zhang, Qi;  Shi, Xuanling;  Wang, Qisheng;  Zhang, Linqi;  Wang, Xinquan
收藏  |  浏览/下载:7/0  |  提交时间:2020/07/03

The measurement sensitivity of quantum probes using N uncorrelated particles is restricted by the standard quantum limit(1), which is proportional to 1/root N. This limit, however, can be overcome by exploiting quantum entangled states, such as spin-squeezed states(2). Here we report the measurement-based generation of a quantum state that exceeds the standard quantum limit for probing the collective spin of 10(11) rubidium atoms contained in a macroscopic vapour cell. The state is prepared and verified by sequences of stroboscopic quantum non-demolition (QND) measurements. We then apply the theory of past quantum states(3,4) to obtain spin state information from the outcomes of both earlier and later QND measurements. Rather than establishing a physically squeezed state in the laboratory, the past quantum state represents the combined system information from these prediction and retrodiction measurements. This information is equivalent to a noise reduction of 5.6 decibels and a metrologically relevant squeezing of 4.5 decibels relative to the coherent spin state. The past quantum state yields tighter constraints on the spin component than those obtained by conventional QND measurements. Our measurement uses 1,000 times more atoms than previous squeezing experiments(5-10), with a corresponding angular variance of the squeezed collective spin of 4.6 x 10(-13) radians squared. Although this work is rooted in the foundational theory of quantum measurements, it may find practical use in quantum metrology and quantum parameter estimation, as we demonstrate by applying our protocol to quantum enhanced atomic magnetometry.


  
Seesaw haze pollution in North China modulated by the sub-seasonal variability of atmospheric circulation 期刊论文
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2019, 19 (1) : 565-576
作者:  Zhang, Ge;  Gao, Yang;  Cai, Wenju;  Leung, L. Ruby;  Wang, Shuxiao;  Zhao, Bin;  Wang, Minghuai;  Shan, Huayao;  Yao, Xiaohong;  Gao, Huiwang
收藏  |  浏览/下载:7/0  |  提交时间:2019/04/09
Laboratory observations of temperature and humidity dependencies of nucleation and growth rates of sub-3nm particles 期刊论文
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2017, 122 (3)
作者:  Yu, Huan;  Dai, Liang;  Zhao, Yi;  Kanawade, Vijay P.;  Tripathi, Sachchida N.;  Ge, Xinlei;  Chen, Mindong;  Lee, Shan-Hu
收藏  |  浏览/下载:5/0  |  提交时间:2019/04/09